arXiv subjects

Delphine Lagarde

Publications and source records attributed to Delphine Lagarde.

At least 19 recordsLinked to original sources

arXiv2026

Entangled Telecom Photon Generation using Twisted Van der Waals Crystals

Nanoscale quantum light sources are essential building blocks for integrated quantum photonic systems. Here, we report a wavelength-scale entangled-photon source based on van der Waals-engineered NbOBr$_2$, and benchmark its performance for telecom-wavelength quantum light generation. By exploiting the material's second-order nonlinearity, we generate quantum-correlated photon pairs via spontaneous parametric down-conversion. We then use a 90$^{\circ}$ twisted stacking to induce quantum interference in photon-pair generation, yielding polarization-entangled photons. This approach enables tunability of the quantum optical state via control of the excitation laser polarization. We experimentally obtain entanglement fidelities exceeding 95% for Bell states, along with a high coincidence-to-accidental ratio of $\sim$335, and a brightness approximately one order of magnitude higher than recently reported telecom sources based on transition metal dichalcogenide (TMD) 2D materials. These results establish twisted van der Waals engineering as a powerful platform for highly tunable, high-brightness quantum light sources at telecom wavelengths.

physics.optics↗

arXiv2026

Sub-nm range momentum-dependent exciton transfer from a 2D semiconductor to graphene

Heterostructures made from atomically thin semiconductors (here MoSe$_2$) and graphene are uniquely poised to investigate photoinduced charge and energy transfer in the 2D limit. Here, using picosecond time-resolved photoluminescence spectroscopy at cryogenic temperatures on two types of MoSe$_2$/graphene heterostrutures, we unveil key features of the underlying mechanisms. First, the shortening of the MoSe$_2$ bright exciton lifetime is marginally affected by the number of graphene layers to which MoSe$_2$ is coupled. Second, exciton transfer vanishes when a sub-nm thick spacer of hexagonal boron nitride decouples MoSe$_2$ from graphene. These results indicate that charge tunneling govern bright exciton relaxation in MoSe$_2$/graphene and that longer-range, F\"orster-type energy transfer (FRET) does not affect bright excitons. However, sub-ps FRET to graphene accelerates the relaxation of ``hot'' excitons formed upon optical excitation, leading to photoluminescence quenching factors that exceed expectations based on the shortening of the bright exciton lifetime. Our work has direct implications for energy harvesting and funneling using van der Waals heterostructures.

cond-mat.mes-hall↗

arXiv2026

Emission Dynamics of Rydberg Excitons in $\mathbf{\mathrm{Cu_2O}}$: Distinguishing Second Harmonic Generation from Secondary Emission

Rydberg excitons in $\mathrm{Cu_2O}$ simultaneously give rise to two very different optical responses under resonant two-photon excitation: a coherent second-harmonic signal mediated by the excitonic second order susceptibility tensor $\chi^{(2)}$, and a secondary emission originating from the radiative decay of real exciton populations. Distinguishing these two channels is essential for interpreting nonlinear and quantum-optical experiments based on high-$n$ states, yet their temporal, spectral, and power-dependent signatures often overlap. Here we use time-resolved resonant two-photon excitation to cleanly separate SHG and SE and to map how each depends on $n$, temperature, excitation power, and crystal quality. This approach reveals the markedly different sensitivities of the two processes to phonons, defects, and many-body effects, and establishes practical criteria for identifying SE and SHG in a wide range of experimental conditions. Our results provide a unified framework for interpreting emission from Rydberg excitons and offer guidelines for future studies aiming to exploit their nonlinear response and long-range interactions.

cond-mat.quant-gas↗

arXiv2025

Non-radiative energy transfer between boron vacancies in hexagonal boron nitride and other 2D materials

Boron vacancies ($V_B^-$) in hexagonal boron nitride (hBN) have emerged as a promising platform for two-dimensional quantum sensors capable of operating at atomic-scale proximity. However, the mechanisms responsible for photoluminescence quenching in thin hBN sensing layers when placed in contact with absorptive materials remain largely unexplored. In this Letter, we investigate non-radiative F\"orster resonance energy transfer (FRET) between $V_B^-$ centers and either monolayer graphene or 2D semiconductors. Strikingly, we find that the FRET rate is negligible for hBN sensing layers thicker than 3 nm, highlighting the potential of $V_B^-$ centers for integration into ultra-thin quantum sensors within van der Waals heterostructures. Furthermore, we experimentally extract the intrinsic radiative decay rate of $V_B^-$ defects.

cond-mat.mtrl-sci↗

arXiv2025

High luminescence efficiency of multi-valley excitonic complexes in heavily doped WSe2 monolayer

Monolayers of group-VI transition-metal dichalcogenides (TMDs) are two-dimensional semiconductors that exhibit exceptionally strong light-matter coupling yet typically suffer from low emission quantum yields. In this letter, we investigate the heavily n-doped regime of a WSe$_2$ monolayer and show that multi-particle excitonic complexes produce photoluminescence signals up to two orders of magnitude stronger than in the neutral state. Time-resolved photoluminescence and differential reflectivity measurements reveal that the quantum yield rises with carrier density and exceeds 50% for electron concentrations above 10$^{13}$ cm$^{-2}$. These findings establish TMD monolayers as a platform for exploring excitonic complexes in high-density electron gases and point toward new opportunities for efficient, atomically thin light emitters.

cond-mat.mes-hall↗

arXiv2025

Thermal assisted transport of biexcitons in monolayer WSe2

Studies of excitonic transport in transition metal dichalcogenide monolayers have attracted increasing interest in recent years in order to develop nano-optoelectronic devices made with 2D materials. These studies began with low to moderate optical excitation regimes, and more recently have focused on high injection regimes where nonlinear effects appear. This article is focused on the transport of biexcitons by spatially and temporally resolved photoluminescence spectroscopy at high excitation flux. The study is carried out on a high-quality WSe$_2$ monolayer encapsulated in hexagonal boron nitride. The results show that a Seebeck current affects transport in connection with the presence of hot biexcitons. In particular, we observe the formation of spatial rings, also called halos, which have been observed in other excitonic gases. These results tend to generalize the importance of high-energy populations in excitonic transport in TMD, even for complex and heavy excitonic particles.

cond-mat.mtrl-sci↗

arXiv2025

Charge state tuning of spin defects in hexagonal boron nitride

Boron vacancies in hexagonal boron nitride (hBN) are among the most extensively studied optically active spin defects in van der Waals crystals, due to their promising potential to develop two-dimensional (2D) quantum sensors. In this letter, we demonstrate the tunability of the charge state of boron vacancies in ultrathin hBN layers, revealing a transition from the optically active singly negatively charged state to the optically inactive doubly negatively charged state when sandwiched between graphene electrodes. Notably, there is a photoluminescence quenching of a few percent upon the application of a bias voltage between the electrodes. Our findings emphasize the critical importance of considering the charge state of optically active defects in 2D materials, while also showing that the negatively charged boron vacancy remains robust against external perpendicular electric fields. This stability makes it a promising candidate for integration into various van der Waals heterostructures.

cond-mat.mtrl-sci↗

arXiv2024

Direct measurement of the lifetime and coherence time of Cu2O Rydberg excitons

Rydberg states of excitons are promising quantum objects to engineer giant nonlinearities in a solid-state system. For this purpose, a deeper understanding of the dynamics of Rydberg excitons and of their potential for coherent manipulation becomes important. We report experimental results where two-photon absorption is resonant with various Rydberg states of excitons in copper oxide and we detect their emission dynamics on a streak camera with sub-picosecond resolution. This technique enables the direct measurement of the Rydberg states lifetimes, which are in good agreement with the expected Rydberg scaling law. Moreover, we observe several intriguing dynamics including the presence of long-lived coherent oscillations. Finally, we independently measure the coherence time of the Rydberg states using a modified Michelson interferometer and find a good agreement with the coherent oscillations detected in the exciton emission dynamics. The lifetimes also reveal the absence of inhomogeneous broadening in the current high-precision spectroscopic data for the S series, which together with the presence of significant coherence time confirms the suitability of the system for coherent engineering.

quant-ph↗

arXiv2024

Using Light to Polarize and Detect Electron Spins in Silicon

Despite decades of research, demonstration of all-optical detection and control of free electron spins in silicon remains elusive. Here, we directly probe the electron spin properties in bulk silicon by measuring the polarization of luminescence following circularly polarized light excitation. The experiments performed for both direct and indirect gap excitation allow not only an experimental determination of the optical selection rules in silicon for the different phononassisted transitions but they also lead to the measurement of the spin relaxation of electrons in conditions which are not accessible using transport techniques. We also measure the spin properties of free excitons in bulk silicon, a very little explored field.

cond-mat.mtrl-sci↗

arXiv2024

Performance of graphene Hall effect sensors: role of bias current, disorder and Fermi velocity

Graphene Hall effect magnetic field sensors hold great promise for the development of ultra-sensitive magnetometers. Their performance is frequently analysed using the two-channel model where electron and hole conductivities are simply added. Unfortunately, this model is unable to capture all the features of the sensor, particularly the bias current dependence of the magnetic field sensitivity. Here we present an advanced model that provides an in-depth understanding of how graphene Hall sensors operate, and demonstrate its ability to quantitatively assess their performance. First, we report the fabrication of sensors with different qualities of graphene, with the best devices achieving magnetic field sensitivities as high as 5000 ohms/T, outperforming the best silicon and narrow-gap semiconductor-based sensors. Then, we examine their performance in detail using the proposed numerical model, which combines Boltzmann formalism, with distinct Fermi levels for electrons and holes, and a new method for the introduction of substrate-induced electron-hole puddles. Importantly, the dependences of magnetic field sensitivity on bias current, disorder, substrate and Hall bar geometry are quantitatively reproduced for the first time. In addition, the model emphasizes that the performance of devices with widths of the order of the charge carrier diffusion length, is significantly affected by the bias current due to the occurrence of large and non-symmetric carrier accumulation and depletion areas near the edges of the Hall bar. The formation of these areas induces a transverse diffusion particle flux capable of counterbalancing the particle flux induced by the Lorentz force when the Hall electric field cancels out in the ambipolar regime. Finally, we discuss how sensor performance can be enhanced by Fermi velocity engineering, paving the way for future ultra-sensitive graphene Hall effect sensors.

cond-mat.mes-hall↗

arXiv2024

Large-scale characterization of Cu2O monocrystals via Rydberg excitons

Rydberg states of excitons can reach microns in size and require extremely pure crystals. We introduce an experimental method for the rapid and spatially-resolved characterization of Rydberg excitons in copper oxide (Cu2O) with sub-micron resolution over large zones. Our approach involves illuminating and imaging the entire sample on a camera to realize a spatially-resolved version of resonant absorption spectroscopy, without any mobile part. This yields spatial maps of Rydberg exciton properties, including their energy, linewidth and peak absorption, providing a comprehensive quality assessment of the entire sample in a single shot. Furthermore, by imaging the sample photoluminescence over the same zone, we establish a strong relationship between the spectral quality map and the photoluminescence map of charged oxygen vacancies. This results in an independent, luminescence-based quality map that closely matches the results obtained through resonant spectroscopy. Our findings reveal that Rydberg excitons in natural Cu2O crystals are predominantly influenced by optically-active charged oxygen vacancies, which can be easily mapped. Together, these two complementary methods provide valuable insights into Cu2O crystal properties.

cond-mat.quant-gas↗

arXiv2023

Kapitza-resistance-like exciton dynamics in atomically flat MoSe$_{2}$-WSe$_{2}$ lateral heterojunction

Being able to control the neutral excitonic flux is a mandatory step for the development of future room-temperature two-dimensional excitonic devices. Semiconducting Monolayer Transition Metal Dichalcogenides (TMD-ML) with extremely robust and mobile excitons are highly attractive in this regard. However, generating an efficient and controlled exciton transport over long distances is a very challenging task. Here we demonstrate that an atomically sharp TMD-ML lateral heterostructure (MoSe$_{2}$-WSe$_{2}$) transforms the isotropic exciton diffusion into a unidirectional excitonic flow through the junction. Using tip-enhanced photoluminescence spectroscopy (TEPL) and a modified exciton transfer model, we show a discontinuity of the exciton density distribution on each side of the interface. We introduce the concept of exciton Kapitza resistance, by analogy with the interfacial thermal resistance referred to as Kapitza resistance. By comparing different heterostructures with or without top hexagonal boron nitride (hBN) layer, we deduce that the transport properties can be controlled, over distances far greater than the junction width, by the exciton density through near-field engineering and/or laser power density. This work provides a new approach for controlling the neutral exciton flow, which is key toward the conception of excitonic devices.

cond-mat.mes-hall↗

arXiv2022

Probing the optical near-field interaction of Mie nanoresonators with atomically thin semiconductors

Optical Mie resonators based on silicon nanostructures allow tuning of light-matter-interaction with advanced design concepts based on CMOS compatible nanofabrication. Optically active materials such as transition-metal dichalcogenide (TMD) monolayers can be placed in the near-field region of such Mie resonators. Here, we experimentally demonstrate and verify by numerical simulations coupling between a MoSe2 monolayer and the near-field of dielectric nanoresonators. Through a comparison of dark-field (DF) scattering spectroscopy and photoluminescence excitation experiments (PLE), we show that the MoSe2 absorption can be enhanced via the near-field of a nanoresonator. We demonstrate spectral tuning of the absorption via the geometry of individual Mie resonators. We show that we indeed access the optical near-field of the nanoresonators, by measuring a spectral shift between the typical near-field resonances in PLE compared to the far-field resonances in DF scattering. Our results prove that using MoSe2 as an active probe allows accessing the optical near-field above photonic nanostructures, without the requirement of highly complex near-field microscopy equipment.

physics.optics↗

arXiv2022

Exciton spectroscopy and diffusion in MoSe2-WSe2 lateral heterostructures encapsulated in hexagonal boron nitride

Chemical vapor deposition (CVD) allows lateral edge epitaxy of transition metal dichalcogenide heterostructures with potential applications in optoelectronics. Critical for carrier and exciton transport is the quality of the two materials that constitute the monolayer and the nature of the lateral heterojunction. Important details of the optical properties were inaccessible in as-grown heterostructure samples due to large inhomogeneous broadening of the optical transitions. Here we perform optical spectroscopy at T = 4 K and also at 300 K to access the optical transitions in CVD grown MoSe2-WSe2 lateral heterostructures that are transferred from the growth-substrate and are encapsulated in hBN. Photoluminescence (PL), reflectance contrast and Raman spectroscopy reveal considerably narrowed optical transition linewidth similar to high quality exfoliated monolayers. In high-resolution transmission electron microscopy (HRTEM) we find near-atomically sharp junctions with a typical extent of 3nm for the covalently bonded MoSe2-WSe2. In PL imaging experiments we find effective excitonic diffusion length that are longer for WSe2 than for MoSe2 at low T=4 K, whereas at 300 K this trend is reversed.

cond-mat.mtrl-sci↗

arXiv2022

Optical detection of long electron spin transport lengths in a monolayer semiconductor

Using a spatially-resolved optical pump-probe experiment, we measure the lateral transport of spin/valley polarized electrons over very long distances (tens of micrometers) in a single WSe2 monolayer. By locally pumping the Fermi sea of 2D electrons to a high degree of spin/valley polarization (up to 75%) using circularly-polarized light, the lateral diffusion of the electron polarization can be mapped out via the photoluminescence induced by a spatially-separated and linearly-polarized probe laser. Up to 25% spin-valley polarization is observed at pump-probe separations up to 20 microns. Characteristic spin/valley diffusion lengths of 18 +/- 3 um are revealed at low temperatures. The dependence on temperature, pump helicity, pump intensity, and electron density highlight the key roles played by spin relaxation time and pumping efficiency on polarized electron transport in monolayer semiconductors possessing spin-valley locking.

cond-mat.mes-hall↗

arXiv2021

Capacitively-coupled and inductively-coupled excitons in bilayer MoS$_2$

The interaction of intralayer and interlayer excitons is studied in a two-dimensional semiconductor, homobilayer MoS$_2$. It is shown that the measured optical susceptibility reveals both the magnitude and the sign of the coupling constants. The interlayer exciton interacts capacitively with the intralayer B-exciton (positive coupling constant) consistent with hole tunnelling from one monolayer to the other. Conversely, the interlayer exciton interacts inductively with the intralayer A-exciton (negative coupling constant). First-principles many-body calculations show that this coupling arises via an intravalley exchange-interaction of A- and B-excitons.

cond-mat.mes-hall↗

arXiv2021

Giant Stark splitting of an exciton in bilayer MoS$_2$

Transition metal dichalcogenides (TMDs) constitute a versatile platform for atomically thin optoelectronics devices and spin-valley memory applications. In monolayers optical absorption is strong, but the transition energy is not tunable as the neutral exciton has essentially no out-of-plane electric dipole. In contrast, interlayer exciton transitions in heterobilayers are widely tunable in applied electric fields, but their coupling to light is considerably reduced. Here, we show tuning over 120 meV of interlayer excitons with high oscillator strength in bilayer MoS2. These shifts are due to the quantum confined Stark effect, here the electron is localised to one of the layers yet the hole is delocalised across the bilayer. We optically probe the interaction between intra- and interlayer excitons as they are energetically tuned into resonance. This allows studying their mixing supported by beyond standard density functional theory calculations including excitonic effects. In MoS2 trilayers our experiments uncover two types of interlayer excitons with and without in-built electric dipoles, respectively. Highly tunable excitonic transitions with large oscillator strength and in-built dipoles, that lead to considerable exciton-exciton interactions, hold great promise for non-linear optics with polaritons.

cond-mat.mes-hall↗

arXiv2021

Interlayer exciton mediated second harmonic generation in bilayer MoS2

Second harmonic generation (SHG) is a non-linear optical process, where two photons coherently combine into one photon of twice their energy. Efficient SHG occurs for crystals with broken inversion symmetry, such as transition metal dichalcogenide monolayers. Here we show tuning of non-linear optical processes in an inversion symmetric crystal. This tunability is based on the unique properties of bilayer MoS2, that shows strong optical oscillator strength for the intra- but also inter-layer exciton resonances. As we tune the SHG signal onto these resonances by varying the laser energy, the SHG amplitude is enhanced by several orders of magnitude. In the resonant case the bilayer SHG signal reaches amplitudes comparable to the off-resonant signal from a monolayer. In applied electric fields the interlayer exciton energies can be tuned due to their in-built electric dipole via the Stark effect. As a result the interlayer exciton degeneracy is lifted and the bilayer SHG response is further enhanced by an additional two orders of magnitude, well reproduced by our model calculations.

cond-mat.mtrl-sci↗